ChemSusChem
·
2021
·Vol. 14
·期 19
·4242-4250
·
IF 8.928
Shenglu Lu,Yaxuan Jing,Bo Feng,Yong Guo,Xiaohui Liu,Yanqin Wang
Graphical Hidden hydrogen : Polyethylene terephthalate (PET) is the most widely used synthetic polyester, and its degradation is increasingly recognized as essential to develop the future provision of energy and reduce environmental pollution. Reported herein is a salient example of H 2 -free conversion of PET back to BTX stream with alkyl aromatics as the main products by unlocking hidden hydrogen in the structural ethylene glycol part in a selective manner. The strong desire for a circular economy makes obtaining fuels and chemicals via plastic degradation an important research topic in the 21st century. Here, the first example of the H 2 -free polyethylene terephthalate (PET) conversion to BTX (benzene, toluene and xylene) was achieved by unlocking hidden hydrogen in the ethylene glycol part over Ru/Nb 2 O 5 catalyst. Among the whole process (hydrolysis, reforming and hydrogenolysis/decarboxylation), the parallel hydrogenolysis and decarboxylation were competing and the rate-determining step. Ru/Nb 2 O 5 exhibited superior hydrogenolysis and poorer decarboxylation performance in direct comparison with Ru/NiAl 2 O 4 , accordingly contributing to the distinct selectivity to alkyl aromatics among BTX. Ru species on Nb 2 O 5 , unlike those on NiAl 2 O 4 , showed more Ru δ + species owing to the strong interaction between Ru and Nb 2 O 5 , restricting the undesired decarboxylation. Along with NbO x species for C−O bond activation, excellent reactivity towards the H 2 -free conversion of PET back to BTX with alkyl aromatics as dominant species was achieved. This H 2 -free system was also capable of converting common real PET plastics back to BTX, adding new options in the circular economy of PET.
研究领域:
化学工程
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环境科学
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催化科学
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产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Zheng Shen,Xindong Zhang,Xiaohui Ma,Ruoning Mi,Yu Chen,Shengping Ruan
A novel hierarchical ZnO rose-like architecture assembled by porous nanosheets was synthesized through a facile hydrothermal method combined with calcination process and used to fabricate gas sensors. The gas sensing measurements showed that the samples exhibited superior individual BTX (benzene, toluene and xylene) sensing properties. By designing more tiny pores on hierarchical rose petal-like nanosheet surface, the specific surface area of the samples was further extended. Besides, highly dispersed Au nanoparticles were grown on the ZnO rose-like architectures to enhance the gas sensing performance via a precipitation manner. Transmission electron microscopy (TEM) analyses indicated the average grain size of these Au nanoparticles was about 3 nm. The gas sensing results showed that the responses of the Au-ZnO sensor to 20 ppm individual benzene, toluene and xylene were 16.25 46.43 and 76.47, which were 4.33, 4.47 and 6.51 times higher than those of the pure specimens. Besides, the optimal working temperature was also decreased from 302 °C to 206 °C. The Au-ZnO sensor also exhibited short response/recovery times, low-concentration detection capability and good stability. The schottky contact between Au and ZnO, catalytic activity of Au nanoparticles and the specific ZnO porous rose-like architectures could be three pivotal factors for the superior BTX sensing properties.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xingxing Cui,Hongyang Lyu,Yongming Chai,Bin Liu,Dongfeng Zhao,Chenguang Liu
The strong acidity on the external surface of ZSM-5 is a primary factor resulting in the low BTX selectivity and catalyst deactivation during the olefin aromatization. In this study, a membrane-restricted Silicalite-1@ZSM-5 core–shell structured catalytic catalyst was designed and constructed for 1-hexene aromatization using a hydrothermal coating method. TEM and NMR results confirmed the complete coverage of Silicalite-1 on the surface of ZSM-5, with a shell thickness of 50 nm. The further reaction of the TIPB (1,3,5-triisopropylbenzene) molecular probe reactions demonstrated the passivation of the acid sites on ZSM-5 external surface. The inert shell layer passivated the acid sites on the external surface, thereby suppressing the isomerization of PX and the side-chain alkylation reaction of light aromatics. Compared to ZSM-5, the Silicalite-1@ZSM-5 catalyst exhibited a 37.15 % increase in BTX selectivity, a 58.65 % increase in PX selectivity, significantly reduced coke deposition, and demonstrated better stability. This strategy of in-situ epitaxial growth of inert shell layers holds significant promise for enhancing the selectivity of shape-selective catalysts and extending catalyst lifetime.
研究领域:
催化化学
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材料科学
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石油化工
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产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Zunlong Hu,Peng Hu,Xiulin Wang,Tongtong Wu,Sida Ge,Haodong Xie,Baijun Liu,Shengli Chen,Zhijie Wu
The hydrocracking catalyst is characteristic of bifunctional catalyst mainly requiring metal–acid balance, which includes metal–acid ratio and metal–acid proximity. Here, we screened and clarified the optimal metal–acid balance on 1-methylnaphthalene (1-MN) hydrocracking by adjusting metal–acid ratio (n M /n A ) via physically mixing the γ-Al 2 O 3 supported NiW samples and Beta zeolite with different acidity (denoted as NiW/AB(x) and x presents the molar ratio of SiO 2 /Al 2 O 3 for Beta zeolite). NiW/AB(60) catalyst with a n M /n A of 0.40 showed the highest BTX selectivity (14.4 %) at a 1-MN conversion of 76.6 %, suggesting an optimal site balance between the metal sulfide site and medium-strong acid sites ( ca . 1:2.5). Also, four different metal–acid proximities with centimeter, millimeter, micrometer and nanoscale distances were compared. The nanoscale proximity enabled the highest BTX selectivity (19.6 %) as compared to the microscale (14.4 %), millimeter scale (12.4 %) and centimeter scale (7.1 %) catalysts, confirming that the selectivity of BTX benefited from the fast diffusion for transporting reaction intermediates between metal and acid sites. Thus, we realized a n M /n A of 0.40 and a nanoscale site proximity for improving the reactivity and selectivity of 1-MN hydrocracking. This work not only presents an elegant showcase of achieving the synergistic effects of bifunctional catalyst, but also provides a rational approach for enhancing the catalytic performance of hydrocracking and beyond.
研究领域:
催化
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化学工程
·
石油化学
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DOI
高影响因子
Advanced Science
·
2023
·
IF 15.1
Siqi Wang,Yuqiong Wang,Long Lin,Zongjie Li,Fengyi Liu,Long Zhu,Jie Chen,Nianrong Zhang,Xinyu Cao,Sunman Ran,Genzheng Liu,Peng Gao,Weiliang Sun,Liang Peng,Jian Zhuang,Hua Meng
The rising incidence of health-endangering obesity constantly calls for more effective treatments. Gastric intramural injection of botulinum neurotoxin A (BTX-A) as a new modality carries great promise yet inconsistent therapeutic efficacy. A layer-specific delivery strategy enabled by dissolving microneedles is hence pioneered to investigate the working site of BTX-A and the resulting therapeutic effects. The drug-loaded tips of the layer-specific gastric paralysis microneedles (LGP-MN) rapidly release and achieve uniform distribution of BTX-A within the designated gastric wall layers. In an obesity rat model, the LGP-MNs not only prove safer than conventional injection, but also demonstrate consistently better therapeutic effects with muscular layer delivery, including 16.23% weight loss (3.06-fold enhancement from conventional injection), 55.20% slower gastric emptying rate, improved liver steatosis, lowered blood lipids, and healthier gut microbiota. Further hormonal study reveals that the elevated production of stomach-derived glucagon-like peptide-1 due to the muscularis-targeting LGP-MN treatment is an important contributor to its unique glucose tolerance-improving effect. This study provides clear indication of the gastric muscularis as the most favorable working site of BTX-A for weight loss and metabolic improvement purposes, and meanwhile suggests that the LGP-MNs could serve as a novel clinical approach to treat obesity and metabolic syndromes.
研究领域:
药理学
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代谢
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胃肠病学
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肥胖研究
·
药物递送系统
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DOI
PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Hengshuo Gu,Ting Zhao,Jian Li,Yufei Gu,Hucheng Ge,Yuke Liu,Fuwei Li,Zhixia Li,Hongfei Lin,Jiangfei Cao
Hierarchical ZSM-5 (Z-40) was synthesized via a simple two-step hydrothermal crystallization without using any organic template. Low-density polyethylene (LDPE) as hydrogen donor was added into the catalytic pyrolysis of cellulose to enhance deoxygenation and the formation of BTX (benzene, toluene, xylene). Cellulose and LDPE showed the strongest synergistic effect at a feed ratio of 1, and the obtained experimental BTX yield (22.9 %) was 52.7 % higher than the theoretical yield (15 %). Co-catalytic pyrolysis (CCP) of two polymers followed similar cracking behavior to CCP of their pyrolysis vapor model compounds (furfural and n -octane), mainly including pyrolysis, catalytic cracking of pyrolysis fragments in external surface and hydrocarbons pool reactions of small cracking fragments in the internal micropores of zeolite. Z-40 showed better catalytic performance than the commercial ZSM-5 (higher BTX yield and less coke deposition) due to the appropriate acidic properties and distinctive pore structure. The optimal condition for CCP of cellulose/LDPE was temperature at 550 °C, feed ratio at 1:1 and catalyst/feed ratio at 2:1, and the achieved BTX yield reached 24.5 % with high BTX selectivity of 86.7 %. This work provided a cost-effective method for synthesis of ZSM-5 and production of high value-added BTX via a green non-oil route.
研究领域:
化学工程
·
能源科学
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DOI
高影响因子
Catalysts
·
2025
·Vol. 16
·期 1
·
IF 4
Haidong Li,Mingjia Liu,Yifang Zhang,Xiu Chen,Kunyi Zheng,Xilong Wang,Penglei Ni,Jun Ma
The selective hydrocracking of polycyclic aromatic hydrocarbons to BTX requires precise control over catalyst porosity and metal–acid balance. Hierarchical porosity, integrating microporous and mesoporous networks, is pivotal for enhancing mass transport and regulating reaction pathways. USY zeolites were engineered to create distinct hierarchical architectures via HCl, urea, and NaOH–surfactant treatments. HCl treatment constructed a gradient pore acidity system, urea treatment enhanced acidity while preserving microporosity, and NaOH–surfactant fabricated ordered mesopores with reduced acidity. The catalyst with the HCl-engineered gradient pore (NiMo/YH-1) achieved a 91% BTX yield at 425 °C in naphthalene hydrocracking, outperforming others. This performance is attributed to its gradient structure that enforces an optimal “hydrogenation-then-cracking” pathway, highlighting the critical role of tailored hierarchical porosity.
研究领域:
催化化学
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石油化工
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材料科学
·
化学反应工程
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产品关联
DOI
高影响因子
Catalysts
·
2019
·Vol. 9
·期 11
·899
·
IF 3.444
Wei Xu,Lijing Gao,Guomin Xiao
Nano-sized HZSM-5 (n-HZSM-5) was synthesized and applied in the aromatization of glycerol. The effects of additives (carboxymethylcellulose sodium, NaCl, sodium alginate, etc.) on the chemical and physic properties of n-HZSM-5 during preparation were investigated. Metal modification was also investigated based on the synthesized n-HZSM-5. The results showed that the addition of carboxymethylcellulose sodium (CMC-Na), NaCl and sodium alginate (SA) led to forming smaller sizes of HZSM-5 and promoted the acid amounts of the catalysts, which increased its catalytic activities for obtaining BTX. The highest BTX yield of ~35% was obtained by SA derived n-HZSM-5, and the life of the catalyst were both obviously promoted by the additives with a highest of ~11 h by γ-(2,3-epoxypropoxy)propytrimethoxysilane (KH-560) derived n-HZSM-5. BTX yields could be improved by 40%by the addition of Zn and Cd in n-HZSM-5 while having little effect on the catalyst life.
研究领域:
催化化学
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纳米材料科学
·
绿色化学
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Jiayao Qi,Yanni Guo,Hanqiong Jia,Binbin Fan,Hang Gao,Bo Qin,Jinghong Ma,Yanze Du,Ruifeng Li
The commercial Y zeolites are widely used in catalytic cracking and hydrocracking in industry, the efficient hydrocracking of polycyclic aromatics is a challenging task in petroleum and coal refining. The acidic zeolite in the hydrocracking bi-functional catalyst dominates largely the product selectivity, so understanding the independent effect of acid sites is favorable to the design of the catalyst. Herein, five industrial HY zeolites with different ratios of Si/Al were applied to tetralin hydrocracking to produce high-value benzene, toluene, and xylenes (BTX) in a high-pressure fixed bed reactor . The result indicated that mesoporous HUSY not only improved the catalytic activity but also exhibited longer-term stability compared with micropore HY. Interestingly, tetralin conversion in the hydrocracking showed a high-similar value when the Si/Al ratio of the zeolites is above 26 with almost identical porous structure , regardless of the distribution of acidity. And the yield of products is associated with the acidity of the HY zeolites, the lower the Si/Al ratio is, the more favorable the monocyclic aromatic hydrocarbons form. Therefore, it is beneficial for the industrial process to reduce the zeolite post-treatment procedure which achieves the high activity and BTX yield in the hydrocracking of tetralin and to abate the cost consumption, although it is still impractical to get rid of the trial-error scheme for the designing of an efficient catalyst in practice.
研究领域:
催化化学
·
石油加工工程
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产品关联
DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2026
·
IF 3.2
Guo Hanxu,Fu Sen,Yuan Hong
Hierarchical zeolites can provide multidimensional spatial networks, thereby holding significant potential as catalysts for BTX production from biomass pyrolysis. In this study, nano-ZSM-5 zeolite (Z X-X ) with a hierarchical pore structure was synthesized using glycine as a growth inhibitor. Due to the exceptional ability of Ni to cleave C–C and C–H bonds, Ni modification was performed on the Z 30-0.2 catalyst. The effects of glycine and Ni loading on the morphology and pore structure of the zeolites were systematically investigated using scanning electron microscopy (SEM), transmission electron microscopy (TEM), and N 2 adsorption–desorption. The results demonstrated that the particle size of 10 wt% Ni-Z 30-0.2 zeolite ranged from 200 to 300 nm, with a BET surface area of 314 m 2 /g and abundant mesopores. The NH 3 -TPD results showed that the acid amount of 10 wt% Ni-Z 30-0.2 was 0.72 mmol/g. The prepared zeolite was employed in a fixed-bed reactor to catalyze the pyrolysis of oleic acid for the production of benzene, toluene, and xylene (BTX). The introduction of metal Ni significantly enhanced the BTX yield. At 500 ℃, the average BTX yield achieved with the 10 wt% Ni-Z 30-0.2 catalyst was 19.4 wt%, which was higher than that of the zeolite without Ni loading.
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产品关联
DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Bing Xu,Minghui Tan,Xuemei Wu,Hailun Geng,Faen Song,Qingxiang Ma,Chunhui Luan,Guohui Yang,Yisheng Tan
Dehydroaromatization of propane to high value-added aromatics, especially benzene, toluene and xylene (BTX), has attracted widespread attention. Many works have been done to improve the catalytic performance of gallium loaded HZSM-5 catalysts. However, there were few reports focused on reducing the cracked by-products, such as methane and ethylene, derived from propane cracking reaction on external Brønsted acidic sites of zeolite. Herein, chemical liquid deposition (CLD) method was adopted to passivate the external strong Brønsted acid of Ga/HZSM-5, aiming to increase the most value-added BTX production by suppressing the undesired propane cracking reaction. The content of deposited SiO 2 on the external surface of zeolite was tunable by varying the amount of liquid deposition reagent and duration time of CLD process. The results showed that an appropriate content of SiO 2 on external surface of catalyst was beneficial to disable the external strong Brønsted acid sites. Due to depressing the undesired propane cracking reaction, BTX selectivity of 55% with propane conversion of 49% was achieved on Ga/Z5-4Si catalyst, higher than those of Ga/HZSM-5. Otherwise, prolonging the duration time of CLD process narrowed the micropore mouth size of zeolite, which could enhance the shape selective effect of Ga/ZSM-5 to increase the proportion of para-xylene in total xylene products.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 37
·21175-21185
·
IF 3.049
Liuyi Pan,Yulong He,Menglong Niu,Yong Dan,Wenhong Li
Ni–M/SiO2 with different binary metals M (M = Ce, Co, Sn, Fe) prepared by an incipient impregnation method was used in the hydrodeoxygenation (HDO) of low-temperature coal tar distillate, which is rich in phenolic compounds. p-Cresol, as a model compound of the distillate, was used to evaluate the activity and selectivity of BTX products on the series of reduced Ni–M/SiO2 catalysts in a fixed bed reactor. The properties of the catalysts were characterized by N2 adsorption–desorption, ICP-AES, XRD, H2-TPR, and XPS. Benzene and toluene as the direct deoxygenation (DDO) products and cyclohexane and methylcyclohexane as the hydrogenolysis (HYD) products were detected to evaluate the selectivity of the path in the deoxygenation process. In this series of catalysts, the order of reactivity was Ni–Ce > Ni–Sn > Ni–Co > Ni–Fe > monometallic Ni. Meanwhile, the addition of Ce and Co loaded in the Lewis acid sites of the catalyst affected the electron distribution of nickel atom and its atomic arrangement on the surface of the carrier. Compared to monometallic Ni, the DDO path become dominant on Ni–Ce and Ni–Co and the selectivity for BTX products increased from 58.8% to 77.4% and 71.1%, respectively. The binary metal Sn, unlike the former two metals, formed a Ni3Sn crystal form with Ni, which resulted in significant enhancement of the HYD path while obviously increasing the reactivity.
研究领域:
化学工程
·
催化材料科学
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DOI
PubMed
高影响因子
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